Strongly correlated perovskite lithium ion shuttles

Journal Article · 13 August 2018 · Proceedings of the National Academy of Sciences of the United States of America

DOI: https://doi.org/10.1073/pnas.1805029115 · OSTI ID:1464333

Sun, Yifei ^[1]; Kotiuga, Michele ^[2]; Lim, Dawgen ^[1]; Narayanan, Badri ^[3]; Cherukara, Mathew ^[4]; Zhang, Zhen ^[1]; Dong, Yongqi ^[4]; Kou, Ronghui ^[4]; Sun, Cheng-Jun ^[4]; Lu, Qiyang ^[5]; Waluyo, Iradwikanari ^[6]; Hunt, Adrian ^[6]; Tanaka, Hidekazu ^[7]; Hattori, Azusa N. ^[7]; Gamage, Sampath ^[8]; Abate, Yohannes ^[8]; Pol, Vilas G.  ^[9]; Zhou, Hua ^[4]; Sankaranarayanan, Subramanian K. R. S. ^[10]; Yildiz, Bilge ^[11] ; Rabe, Karin M. ^[2]; Ramanathan, Shriram ^[1]

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1. School of Materials Engineering, Purdue University, West Lafayette, IN 47907,
2. Department of Physics and Astronomy, Rutgers, The State University of New Jersey, Piscataway, NJ 08854,
3. Materials Science Division, Argonne National Laboratory, Argonne, IL 60439,
4. X-Ray Science Division, Advanced Photon Source, Argonne National Laboratory, Argonne, IL 60439,
5. Laboratory for Electrochemical Interfaces, Massachusetts Institute of Technology, Cambridge, MA 02139,, Department of Materials Science and Engineering, Massachusetts Institute of Technology, Cambridge, MA 02139,
6. National Synchrotron Light Source II, Brookhaven National Laboratory, Upton, NY 11973,
7. Institute of Scientific and Industrial Research, Osaka University, Osaka 567-0047, Japan,
8. Department of Physics and Astronomy, University of Georgia, Athens, GA 30602,
9. Davidson School of Chemical Engineering, Purdue University, West Lafayette, IN 47907,
10. Center for Nanoscale Materials, Argonne National Laboratory, Argonne, IL 60439,
11. Laboratory for Electrochemical Interfaces, Massachusetts Institute of Technology, Cambridge, MA 02139,, Department of Materials Science and Engineering, Massachusetts Institute of Technology, Cambridge, MA 02139,, Department of Nuclear Science and Engineering, Massachusetts Institute of Technology, Cambridge, MA 02139

Solid-state ion shuttles are of broad interest in electrochemical devices, nonvolatile memory, neuromorphic computing, and biomimicry utilizing synthetic membranes. Traditional design approaches are primarily based on substitutional doping of dissimilar valent cations in a solid lattice, which has inherent limits on dopant concentration and thereby ionic conductivity. Here, we demonstrate perovskite nickelates as Li-ion shuttles with simultaneous suppression of electronic transport via Mott transition. Electrochemically lithiated SmNiO ₃ (Li-SNO) contains a large amount of mobile Li ⁺ located in interstitial sites of the perovskite approaching one dopant ion per unit cell. A significant lattice expansion associated with interstitial doping allows for fast Li ⁺ conduction with reduced activation energy. We further present a generalization of this approach with results on other rare-earth perovskite nickelates as well as dopants such as Na ⁺ . The results highlight the potential of quantum materials and emergent physics in design of ion conductors.

• Sponsoring Organization: USDOE
• Grant/Contract Number: SC0012704; AC02-06CH11357
• OSTI ID: 1464333
• Journal Information: Proceedings of the National Academy of Sciences of the United States of America, Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Issue: 39 Vol. 115; ISSN 0027-8424
• Publisher: Proceedings of the National Academy of SciencesCopyright Statement
• Country of Publication: United States
• Language: English